A nonlinearity in the magnetoelectric coefficient, αMENonlin, of Metglas/Pb(Zr,Ti)O3 (PZT) and Metglas/Pb(Mg1/3,Nb2/3)O3-PbTiO3 (PMN-PT) laminate sensors has been observed. This nonlinearity was found to be dependent on the dc magnetic bias (Hdc) and frequency of the ac drive field (Hac). The maximum value of αMENonlin for both types of composites was found near the electromechanical resonance. For Metglas/PZT laminates, the maximum occurred under a finite bias of Hdc ≈5 Oe; whereas, for Metglas/PMN-PT, the maximum was found near zero dc bias. One application for αMENonlin is a cross-modulation scheme that can shift low frequency signals to higher frequency to achieve lower noise floor. For Metglas/PMN-PT, αMENonlin has another application: removal of the necessity of a dc bias, which helps to design high-sensitivity sensor arrays and gradiometers.